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Molecular Au(I) complexes in the photosensitized photocatalytic CO2 reduction reaction

Published online by Cambridge University Press:  31 March 2020

Shakeyia Davis
Affiliation:
Department of Chemistry and Biochemistry, University of Mississippi, University, MS38677, USA
Dinesh Nugegoda
Affiliation:
Department of Chemistry and Biochemistry, University of Mississippi, University, MS38677, USA
Joshua Tropp
Affiliation:
School of Polymer Science and Engineering, University of Southern Mississippi, Hattiesburg, MS39406, USA
Jason D. Azoulay
Affiliation:
School of Polymer Science and Engineering, University of Southern Mississippi, Hattiesburg, MS39406, USA
Jared H. Delcamp*
Affiliation:
Department of Chemistry and Biochemistry, University of Mississippi, University, MS38677, USA
*
Address all correspondence to Jared H. Delcamp at [email protected]
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Abstract

Five Au complexes are evaluated for the reduction reaction of CO2 via cyclic voltammetry and in a photocatalytic system. Electrochemically, the complexes were all evaluated for pre-association with CO2 prior to electrochemical reduction and for thermodynamic favorability for CO2 reduction in photocatalytic systems. The complexes were evaluated in photocatalytic reactions using an Ir-based photosensitizer and a sacrificial electron donor for the conversion of CO2 to CO. Au-complex counterion effects on the photocatalytic reaction were analyzed by varying weakly coordinating counterions with significant performance changes noted. At low Au-complex concentrations, a high TON value of 700 was observed.

Type
Research Letters
Copyright
Copyright © Materials Research Society 2020

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References

1.Jupally, V.R., Dharmaratne, A.C., Crasto, D., Huckaba, A.J., Kumara, C., Nimmala, P.R., Kothalawala, N., Delcamp, J.H., and Dass, A.: Au137(SR)56 nanomolecules: composition, optical spectroscopy, electrochemistry and electrocatalytic reduction of CO2. Chem. Commun. 50, 9895 (2014).CrossRefGoogle Scholar
2.Kauffman, D.R., Alfonso, D., Matranga, C., Qian, H., and Jin, R.: Experimental and computational investigation of Au25 clusters and CO2: a unique interaction and enhanced electrocatalytic activity. J. Am. Chem. Soc. 134, 10237 (2012).CrossRefGoogle ScholarPubMed
3.Chen, Y., Li, C.W., and Kanan, M.W.: Aqueous CO2 reduction at very low overpotential on oxide-derived Au nanoparticles. J. Am. Chem. Soc. 134, 19969 (2012).CrossRefGoogle ScholarPubMed
4.Sun, K., Cheng, T., Wu, L., Hu, Y., Zhou, J., Maclennan, A., Jiang, Z., Gao, Y., Goddard, W.A. 3rd, and Wang, Z.: Ultrahigh mass activity for carbon dioxide reduction enabled by gold-iron core-shell nanoparticles. J. Am. Chem. Soc. 139, 15608 (2017).CrossRefGoogle ScholarPubMed
5.Kim, H., Park, H.S., Hwang, Y.J., and Min, B.K.: Surface-morphology-dependent electrolyte effects on gold-catalyzed electrochemical CO2 reduction. J. Phys. Chem. C 121, 22637 (2017).CrossRefGoogle Scholar
6.Huckaba, A.J., Sharpe, E.A., and Delcamp, J.H.: Photocatalytic reduction of CO2 with Re-Pyridyl-NHCs. Inorg. Chem. 55, 682 (2016).CrossRefGoogle ScholarPubMed
7.Cope, J.D., Liyanage, N.P., Kelley, P.J., Denny, J.A., Valente, E.J., Webster, C.E., Delcamp, J.H., and Hollis, T.K.: Electrocatalytic reduction of CO2 with CCC-NHC pincer nickel complexes. Chem. Commun. 53, 9442 (2017).CrossRefGoogle ScholarPubMed
8.Das, S., Rodrigues, R.R., Lamb, R.W., Qu, F., Reinheimer, E., Boudreaux, C.M., Webster, C.E., Delcamp, J.H., and Papish, E.T.: Highly active ruthenium CNC pincer photocatalysts for visible-light-driven carbon dioxide reduction. Inorg. Chem. 58, 8012 (2019).CrossRefGoogle ScholarPubMed
9.Rodrigues, R.R., Boudreaux, C.M., Papish, E.T., and Delcamp, J.H.: Photocatalytic reduction of CO2 to CO and formate: do reaction conditions or ruthenium catalysts control product selectivity? ACS Appl. Energy Mater. 2, 37 (2019).CrossRefGoogle Scholar
10.Liyanage, N.P., Dulaney, H.A., Huckaba, A.J., Jurss, J.W., and Delcamp, J.H.: Electrocatalytic reduction of CO2 to CO with Re-Pyridyl-NHCs: proton source influence on rates and product selectivities. Inorg. Chem. 55, 6085 (2016).CrossRefGoogle ScholarPubMed
11.Schmidt, M.H., Miskelly, G.M., and Lewis, N.S.: Effects of redox potential, steric configuration, solvent, and alkali metal cations on the binding of carbon dioxide to cobalt(I) and nickel(I) macrocycles. J. Am. Chem. Soc. 112, 3420 (1990).CrossRefGoogle Scholar
12.Agarwal, J., Shaw, T.W., Stanton, C.J. 3rd, Majetich, G.F., Bocarsly, A.B., and Schaefer, H.F. 3rd: NHC-containing manganese(I) electrocatalysts for the two-electron reduction of CO2. Angew. Chem. Int. Ed. 53, 5152 (2014).Google ScholarPubMed
13.Jin, T., He, D., Li, W., Stanton, C.J., Pantovich, S.A., Majetich, G.F., Schaefer, H.F., Agarwal, J., Wang, D., and Li, G.: CO2 reduction with Re(I)-NHC compounds: driving selective catalysis with a silicon nanowire photoelectrode. Chem. Commun. 52, 14258 (2016).CrossRefGoogle ScholarPubMed
14.Stanton, C.J. 3rd, Machan, C.W., Vandezande, J.E., Jin, T., Majetich, G.F., Schaefer, H.F. 3rd, Kubiak, C.P., Li, G., and Agarwal, J.: Re(I) NHC complexes for electrocatalytic conversion of CO2. Inorg. Chem. 55, 3136 (2016).CrossRefGoogle ScholarPubMed
15.Stanton, C.J. 3rd, Vandezande, J.E., Majetich, G.F., Schaefer, H.F. 3rd, and Agarwal, J.: Mn-NHC electrocatalysts: increasing π acidity lowers the reduction potential and increases the turnover frequency for CO2 reduction. Inorg. Chem. 55, 9509 (2016).CrossRefGoogle ScholarPubMed
16.Carpenter, C.A., Brogdon, P., McNamara, L.E., Tschumper, G.S., Hammer, N.I., and Delcamp, J.H.: A robust pyridyl-NHC-ligated rhenium photocatalyst for CO2 reduction in the presence of water and oxygen. Inorganics 6, 22 (2018).CrossRefGoogle Scholar
17.Kuramochi, Y., Ishitani, O., and Ishida, H.: Reaction mechanisms of catalytic photochemical CO2 reduction using Re(I) and Ru(II) complexes. Coord. Chem. Rev. 373, 333 (2018).CrossRefGoogle Scholar
18.Liyanage, N.P., Yang, W., Guertin, S., Sinha Roy, S., Carpenter, C.A., Adams, R.E., Schmehl, R.H., Delcamp, J.H., and Jurss, J.W.: Photochemical CO2 reduction with mononuclear and dinuclear rhenium catalysts bearing a pendant anthracene chromophore. Chem. Commun. 55, 993 (2019).CrossRefGoogle ScholarPubMed
19.Bonin, J., Robert, M., and Routier, M.: Selective and efficient photocatalytic CO2 reduction to CO using visible light and an iron-based homogeneous catalyst. J. Am. Chem. Soc. 136, 16768 (2014).CrossRefGoogle Scholar
20.Widegren, J.A., and Finke, R.G.: A review of the problem of distinguishing true homogeneous catalysis from soluble or other metal-particle heterogeneous catalysis under reducing conditions. J. Mol. Cat. A: Chem. 198, 317 (2003).CrossRefGoogle Scholar
21.Shirley, H., Su, X., Sanjanwala, H., Talukdar, K., Jurss, J.W., and Delcamp, J.H.: Durable solar-powered systems with Ni-catalysts for conversion of CO2 or CO to CH4. J. Am. Chem. Soc. 141, 6617 (2019).CrossRefGoogle ScholarPubMed
22.Thoi, V.S., Kornienko, N., Margarit, C.G., Yang, P., and Chang, C.J.: Visible-light photoredox catalysis: selective reduction of carbon dioxide to carbon monoxide by a nickel N-heterocyclic carbene-isoquinoline complex. J. Am. Chem. Soc. 135, 14413 (2013).CrossRefGoogle ScholarPubMed
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